Toward Efficient and Accurate Prediction of Phonon‐Limited Carrier Mobility by First Principles

Abstract Carrier mobility refers to the ability of charge carriers to move through a material in response to an applied electric field, which has a significant effect on the performance of electronic devices. Understanding and predicting carrier mobility is a fundamental yet difficult subject from a theoretical and computational perspective. In this study, the theory and first‐principles calculation methods for determining carrier mobility are reviewed. The Boltzmann transport theory and its various approximations are introduced, as well as ab initio implementations and some common analytical models for electron‒phonon coupling (EPC), which is the most important factor limiting carrier mobility. Within this theoretical framework, landmark studies on predicting the mobility of 2D materials are surveyed. Additionally, polaron transport at strong EPCs beyond Boltzmann theory is discussed. This review contains up‐to‐date related advances, including magnetotransport calculations, long‐range electron‒dynamical quadrupole coupling, machine‐learning accelerated prediction of EPC matrix elements, high‐throughput screening of high‐mobility materials, and first‐principles polaron calculations. It is aspired that this review will keep condensed matter theorists abreast of the latest advancements in transport theories and first‐principles methods while also empowering users of first‐principles calculation packages to predict transport properties correctly by fostering an understanding of the underlying physical mechanisms.